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The molecular spin state of NiII porphyrin, supported on a ferromagnetic Co surface, can be reversibly switched between spin‐off (S=0) and spin‐on (S=1) states upon coordination and decoordination of the gaseous ligand NH3, respectively (see picture). This finding clearly indicates the possible use of the system as a single‐molecule‐based magnetochemical sensor and in spintronics.

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